当前位置:
X-MOL 学术
›
J. Phys. Chem. Lett.
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Electrochemical Nitrate Reduction Catalyzed by Two-Dimensional Transition Metal Borides
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-02-12 , DOI: 10.1021/acs.jpclett.4c00054
William A Goddard 1 , Charles B Musgrave 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-02-12 , DOI: 10.1021/acs.jpclett.4c00054
William A Goddard 1 , Charles B Musgrave 1
Affiliation
![]() |
We investigated 2D transition metal borides (MBenes) for the efficient conversion of nitrate to ammonia. MBenes have been previously shown to bind oxygen with extraordinary strength, which should translate toward selective adsorption of nitrate in aqueous media. Using Density Functional Theory, we screened MBenes by computing their nitrate and water adsorption energies, seeking materials with strong nitrate binding and weak water binding. We identified MnB, CrB, and VB as the best materials for selective nitrate adsorption and proceeded by computing their free energies for generating ammonia. Of the three candidates, CrB requires the lowest overpotential, making it the best candidate. To further decrease the overpotential, we doped the CrB MBene with secondary transition metals and found the addition of Mn to the active site further reduced the overpotential. We then computed the reaction mechanism grand canonically to observe the effect of applied potential on the free energy landscape.
中文翻译:
二维过渡金属硼化物催化电化学硝酸盐还原
我们研究了二维过渡金属硼化物(MBenes)如何将硝酸盐有效转化为氨。此前,MBenes 已被证明能够以非凡的强度结合氧气,这应该转化为水介质中硝酸盐的选择性吸附。利用密度泛函理论,我们通过计算 MBene 的硝酸盐和水吸附能来筛选 MBene,寻找具有强硝酸盐结合和弱水结合的材料。我们确定 MnB、CrB 和 VB 是选择性硝酸盐吸附的最佳材料,并计算它们产生氨的自由能。在三个候选者中,CrB 需要最低的过电势,使其成为最佳候选者。为了进一步降低过电势,我们在 CrB MBene 中掺杂了二次过渡金属,发现在活性位点添加 Mn 进一步降低了过电势。然后,我们按照标准计算了反应机制,以观察施加电势对自由能景观的影响。
更新日期:2024-02-12
中文翻译:

二维过渡金属硼化物催化电化学硝酸盐还原
我们研究了二维过渡金属硼化物(MBenes)如何将硝酸盐有效转化为氨。此前,MBenes 已被证明能够以非凡的强度结合氧气,这应该转化为水介质中硝酸盐的选择性吸附。利用密度泛函理论,我们通过计算 MBene 的硝酸盐和水吸附能来筛选 MBene,寻找具有强硝酸盐结合和弱水结合的材料。我们确定 MnB、CrB 和 VB 是选择性硝酸盐吸附的最佳材料,并计算它们产生氨的自由能。在三个候选者中,CrB 需要最低的过电势,使其成为最佳候选者。为了进一步降低过电势,我们在 CrB MBene 中掺杂了二次过渡金属,发现在活性位点添加 Mn 进一步降低了过电势。然后,我们按照标准计算了反应机制,以观察施加电势对自由能景观的影响。